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Title: Enhancement of interlayer exchange in an ultrathin two-dimensional magnet

Abstract

Following the recent isolation of monolayer CrI 3, many more two-dimensional van der Waals magnetic materials have been isolated. Their incorporation in van der Waals heterostructures offers a new platform for spintronics, proximity magnetism and quantum spin liquids. A primary question in this field is how exfoliating crystals to the few-layer limit influences their magnetism. Studies of CrI 3 have shown a different magnetic ground state for ultrathin exfoliated films compared with the bulk, but the origin is not yet understood. Here, we use electron tunnelling through few-layer crystals of the layered antiferromagnetic insulator CrCl 3 to probe its magnetic order and find a tenfold enhancement of the interlayer exchange compared with bulk crystals. Moreover, temperature- and polarization-dependent Raman spectroscopy reveals that the crystallographic phase transition of bulk crystals does not occur in exfoliated films. This results in a different low-temperature stacking order and, we hypothesize, increased interlayer exchange. In conclusion, our study provides insight into the connection between stacking order and interlayer interactions in two-dimensional magnets, which may be relevant for correlating stacking faults and mechanical deformations with the magnetic ground states of other more exotic layered magnets such as RuCl 3.

Authors:
 [1];  [1];  [2];  [3]; ORCiD logo [3];  [4]; ORCiD logo [5];  [4];  [6]; ORCiD logo [1]; ORCiD logo [1]
  1. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept.of Physics
  2. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Materials Science and Engineering
  3. Harvard Univ., Cambridge, MA (United States). Dept. of Physics
  4. Ames Lab. and Iowa State Univ., Ames, IA (United States). Dept. of Physics and Astronomy
  5. Ames Lab. and Iowa State Univ., Ames, IA (United States). Dept. of Physics and Astronomy; Univ. Federal do ABC, Santo André, SP (Brazil)
  6. Harvard Univ., Cambridge, MA (United States). Dept. of Physics, and John A. Paulson School of Engineering and Applied Sciences
Publication Date:
Research Org.:
Ames Laboratory (AMES), Ames, IA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); Gordon and Betty Moore Foundation (GBMF); National Science Foundation (NSF); US Army Research Office (ARO)
OSTI Identifier:
1562529
Report Number(s):
IS-J-9986
Journal ID: ISSN 1745-2473
Grant/Contract Number:  
GBMF4541; SC0018935; DMR-1231319; W911NF-14-0247; AC02-07CH11358
Resource Type:
Accepted Manuscript
Journal Name:
Nature Physics
Additional Journal Information:
Journal Name: Nature Physics; Journal ID: ISSN 1745-2473
Publisher:
Nature Publishing Group (NPG)
Country of Publication:
United States
Language:
English

Citation Formats

Klein, Dahlia R., MacNeill, David, Song, Qian, Larson, Daniel T., Fang, Shiang, Xu, Mingyu, Ribeiro, R. A., Canfield, P. C., Kaxiras, Efthimios, Comin, Riccardo, and Jarillo-Herrero, Pablo. Enhancement of interlayer exchange in an ultrathin two-dimensional magnet. United States: N. p., 2019. Web. doi:10.1038/s41567-019-0651-0.
Klein, Dahlia R., MacNeill, David, Song, Qian, Larson, Daniel T., Fang, Shiang, Xu, Mingyu, Ribeiro, R. A., Canfield, P. C., Kaxiras, Efthimios, Comin, Riccardo, & Jarillo-Herrero, Pablo. Enhancement of interlayer exchange in an ultrathin two-dimensional magnet. United States. doi:10.1038/s41567-019-0651-0.
Klein, Dahlia R., MacNeill, David, Song, Qian, Larson, Daniel T., Fang, Shiang, Xu, Mingyu, Ribeiro, R. A., Canfield, P. C., Kaxiras, Efthimios, Comin, Riccardo, and Jarillo-Herrero, Pablo. Mon . "Enhancement of interlayer exchange in an ultrathin two-dimensional magnet". United States. doi:10.1038/s41567-019-0651-0.
@article{osti_1562529,
title = {Enhancement of interlayer exchange in an ultrathin two-dimensional magnet},
author = {Klein, Dahlia R. and MacNeill, David and Song, Qian and Larson, Daniel T. and Fang, Shiang and Xu, Mingyu and Ribeiro, R. A. and Canfield, P. C. and Kaxiras, Efthimios and Comin, Riccardo and Jarillo-Herrero, Pablo},
abstractNote = {Following the recent isolation of monolayer CrI3, many more two-dimensional van der Waals magnetic materials have been isolated. Their incorporation in van der Waals heterostructures offers a new platform for spintronics, proximity magnetism and quantum spin liquids. A primary question in this field is how exfoliating crystals to the few-layer limit influences their magnetism. Studies of CrI3 have shown a different magnetic ground state for ultrathin exfoliated films compared with the bulk, but the origin is not yet understood. Here, we use electron tunnelling through few-layer crystals of the layered antiferromagnetic insulator CrCl3 to probe its magnetic order and find a tenfold enhancement of the interlayer exchange compared with bulk crystals. Moreover, temperature- and polarization-dependent Raman spectroscopy reveals that the crystallographic phase transition of bulk crystals does not occur in exfoliated films. This results in a different low-temperature stacking order and, we hypothesize, increased interlayer exchange. In conclusion, our study provides insight into the connection between stacking order and interlayer interactions in two-dimensional magnets, which may be relevant for correlating stacking faults and mechanical deformations with the magnetic ground states of other more exotic layered magnets such as RuCl3.},
doi = {10.1038/s41567-019-0651-0},
journal = {Nature Physics},
number = ,
volume = ,
place = {United States},
year = {2019},
month = {9}
}

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